Bose, Shameek2015-04-022015-04-022014-12https://hdl.handle.net/11299/170915University of Minnesota Ph.D. dissertation. December 2014. Major: Material Science and Engineering. Advisor: Chris Leighton. 1 computer file (PDF); xv, 156 pages.Thin films and heterostructures of the perovskite cobaltites are of great interest, not only from the point of view of fundamental physics and materials science, but also for technological applications such as solid oxide fuel cells and gas membranes. Their properties are, however, severely deteriorated from the bulk, being dominated by the presence of interfacial "dead layers". Working with the prototypical SrTiO3 (001)/La1-xSrxCoO3 (LSCO) system, our group recently discovered that this degradation in the magnetism and electronic transport at the interface is caused by nanoscopic magneto-electronic phase separation. This was shown to occur primarily due to accumulation of oxygen vacancies near the interface, driven by the interplay between the strain state and the ordering of oxygen vacancies. In the present work we show how this understanding allows for engineering of the interfacial magnetic and electronic transport properties via manipulation of this oxygen vacancy superstructure. We first demonstrate a synthesis technique that utilizes a unique high pressure oxygen plasma to sputter LSCO thin films over a wide doping range 0.05  x  0.80. Then, using reciprocal space mapping and transmission electron microscopy, we demonstrate the ability to control, via the vacancy ordering, the critical strain relaxation thickness by changing the sign of the strain (from tensile on SrTiO3 to compressive on LaAlO3) and crystallographic orientation ((001) vs. (110)). We then provide cross sectional electron energy loss spectroscopy data to show that this strain and orientation control preserves both oxygen and hole carrier concentration at the LaAlO3(001)/LSCO and SrTiO3(110)/LSCO interfaces, strikingly different to the severely depleted SrTiO3(001)/LSCO interface. SQUID magnetometry, polarized neutron reflectometry (PNR) and magneto-transport confirm the concomitant mitigation of the interfacial degradation for LSCO films grown on LaAlO3(001) and SrTiO3(110), as compared to films grown on SrTiO3 (001). Finally, we use scanning tunneling microscopy to provide direct real space images of the magneto-electronic phase separation in ultrathin LSCO on SrTiO3(001). Our work thus demonstrates the ability to utilize oxygen vacancy ordering as a tunable control parameter to tailor interfacial electronic and magnetic properties, with profound implications for the myriad other systems that exhibit unique properties due to such ordering.enCobaltiteInterfaceMagnetismOxygen vacancy orderingStrainThin filmMaterial science and engineeringThesis or Dissertation